Isolated Pd atom anchoring endows cobalt diselenides with regulated water-reduction kinetics for alkaline hydrogen evolution

Isolated Pd atom anchoring endows cobalt diselenides with regulated water-reduction kinetics for alkaline hydrogen evolution
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DOI:
10.1016/j.apcatb.2021.120280
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发表时间:
2021
影响因子:
22.1
通讯作者:
Xu Zhao;Xiangyang Li;Dongdong Xiao;Mingxing Gong;Lulu An;P. Gao;Jinlong Yang;Deli Wang
Xu Zhao;Xiangyang Li;Dongdong Xiao;Mingxing Gong;Lulu An;P. Gao;Jinlong Yang;Deli Wang
中科院分区:
化学1区
文献类型:
--
作者:
Xu Zhao;Xiangyang Li;Dongdong Xiao;Mingxing Gong;Lulu An;P. Gao;Jinlong Yang;Deli Wang

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水的吸附和解离以及氢的吸附是碱性析氢反应(HER)催化过程中的三个关键过程。同时调节这三个过程,以实现催化剂在碱性电解质中的高性能HER,仍然是一个很大的挑战。在此,我们展示了一种简单的方法来合成分离的Pd原子锚定CoSe2(Pd1-CoSe2)纳米带,并协同调节碱性HER的反应过程。机理研究表明,孤立的钯原子锚定在pd1 - cose2上,由于表面位置的带中心向上移动,可以有力地促进水的吸附和解离。同时,钯原子与cose2之间的强相互作用使氢在Pd1-CoSe2上的选择性吸附成为可能。因此,相对于纯CoSe2, pd1 -CoSe2显示出明显的电流增加和向碱性HER的塔菲尔斜率大大降低。该策略为设计具有协同调节反应动力学的多相电催化活性催化剂提供了一种原子级调节策略。
The adsorption and dissociation of water as well as hydrogen adsorption represent three crucial processes in alkaline hydrogen evolution reaction (HER) catalysis. It is still a big challenge to simultaneously regulate these three processes to realize high-performance HER of catalysts in alkaline electrolytes. Herein, we demonstrate a facile approach to synthesize isolated Pd atom-anchored CoSe2(Pd1-CoSe2) nanobelts with synergistically regulated reaction processes for alkaline HER. Mechanistic studies reveal that the anchoring of isolated Pd atoms in Pd1-CoSe2can powerfully promote the adsorption and dissociation of water owing to the upward shiftedd-band center of surface sites. Meanwhile, the strong interactions between Pd atoms and CoSe2enable the well-tailored adsorption of hydrogen on Pd1-CoSe2. Accordingly, relative to pure CoSe2, Pd1-CoSe2shows a remarkably increased current and a much-lowered Tafel slope towards alkaline HER. This strategy provides an atomic-level-regulating strategy to design active catalysts with synergistically regulated reaction kinetics for heterogeneous electrocatalysis.